The electrical conductivity of the organic Mott insulator ET-F2TCNQ (ET = bis(ethylenedithio)tetrathiafulvalene, F2TCNQ = 2,5-difluoro-7,7,8,8-tetracyanoquinodimethane) crystal was found to be enhanced by conjugation with a tetrathiafulvalene (TTF) single crystal on its surface; surface sheet resistance decreased from 5 × l05 to 2 × 103 Ω/sq. The mechanism of this decrement was investigated through optical and atomic force microscopy measurements at the interface. When TTF was conjugated to the ET-F2TCNQ crystal, electron injection from TTF and complex formation between TTF and F2TCNQ occurred. Neutral ET molecules were consequently generated at the interface, and this charge doping broke the Mott insulating state.